When in a quantum optical system the coupling between matter and cavity mode becomes comparable to the bare excitation frequency, we enter a non-perturbative coupling regime, as perturbation theory fails describing the system’s dynamics. While recent advances in Cavity Quantum Electrodynamics allowed to achieve very high values of the coupling strength, thanks to the resonators properties optimization and the employment of solid-state devices, an ever growing interest has been shown about the possibility of significantly modify materials’ properties. It has been demonstrated that the chemical structure of molecules strongly coupled to a photon mode can be altered, which opens the possibility to manipulate and control chemical reactions. The aim of this thesis is to explore non-perturbative regimes on several quantum systems, and to investigate the effects of the coupling upon their properties, such as internal degrees of freedom or electronic states structure. I first developed a novel theory to determine the polariton spectrum of a dipolar ensamble in which a Ising-like dipole-dipole interaction in the 2 non-perturbative regime is considered. A further important focus is the investigation of the saturation effects due to the inclusion of the inter-dipole interaction, and the interplay between the latter and light-matter coupling strength. I also explored specifically the influence of the coupling on the rotational degrees of freedom of an ensemble of two-dimensional freely rotating dipoles, all coupled to a single cavity mode, finding that they are driven by the collective light-matter coupling to undergo a crossover between an isotropic and an aligned phase. I then investigated the case of cavity-embedded doped quantum wells, demonstrating that not only it is possible to couple a discrete cavity mode and bound-to-continuum transitions, but also that a novel bound exciton state appears, induced by the coupling strength. This results shows how light–matter coupling can be used to tune both optical and electronic properties of semiconductor heterostructures beyond those permitted by mere crystal properties. Finally, I explored the physics of an array of THz metamaterial resonators coupled to cyclotron resonances of a two-dimensional electron gas, developing a multiple-mode theory that takes in account the interaction between multiple photon modes mediated by the electrons. My results show that this cross-interaction, due to the strong two-dimensional geometry of the optically active medium, leads to the hybridization of different uncoupled photon modes, and manifests as a visible change of the distribution of the coupled electromagnetic field.
When in a quantum optical system the coupling between matter and cavity mode becomes comparable to the bare excitation frequency, we enter a non-perturbative coupling regime, as perturbation theory fails describing the system’s dynamics. While recent advances in Cavity Quantum Electrodynamics allowed to achieve very high values of the coupling strength, thanks to the resonators properties optimization and the employment of solid-state devices, an ever growing interest has been shown about the possibility of significantly modify materials’ properties. It has been demonstrated that the chemical structure of molecules strongly coupled to a photon mode can be altered, which opens the possibility to manipulate and control chemical reactions. The aim of this thesis is to explore non-perturbative regimes on several quantum systems, and to investigate the effects of the coupling upon their properties, such as internal degrees of freedom or electronic states structure. I first developed a novel theory to determine the polariton spectrum of a dipolar ensamble in which a Ising-like dipole-dipole interaction in the 2 non-perturbative regime is considered. A further important focus is the investigation of the saturation effects due to the inclusion of the inter-dipole interaction, and the interplay between the latter and light-matter coupling strength. I also explored specifically the influence of the coupling on the rotational degrees of freedom of an ensemble of two-dimensional freely rotating dipoles, all coupled to a single cavity mode, finding that they are driven by the collective light-matter coupling to undergo a crossover between an isotropic and an aligned phase. I then investigated the case of cavity-embedded doped quantum wells, demonstrating that not only it is possible to couple a discrete cavity mode and bound-to-continuum transitions, but also that a novel bound exciton state appears, induced by the coupling strength. This results shows how light–matter coupling can be used to tune both optical and electronic properties of semiconductor heterostructures beyond those permitted by mere crystal properties. Finally, I explored the physics of an array of THz metamaterial resonators coupled to cyclotron resonances of a two-dimensional electron gas, developing a multiple-mode theory that takes in account the interaction between multiple photon modes mediated by the electrons. My results show that this cross-interaction, due to the strong two-dimensional geometry of the optically active medium, leads to the hybridization of different uncoupled photon modes, and manifests as a visible change of the distribution of the coupled electromagnetic field.
In modern physics, the investigation of the interaction between light and matter is important from both a fundamental and an applied point of view. Cavity quantum electrodynamics (cavity QED) is the study of the interaction between light confined in a reflective cavity and atoms or other particles where the quantum nature of light photons is significant. The strong interaction between an exciton and cavity photon in a high-finesse microcavity can induce a hybrid light-matter eigenstate which is usually named as polariton in solid-state systems. This strong light-matter interaction can be achieved when this interaction is larger than all broadenings caused by other various factors e.g. electron phonon scattering and cavity loss. The polariton is now stimulating tremendous research interests due to its high potential in cavity quantum electrodynamics (QED) and the achievement of polaritonic devices. Moreover, when the interaction strength between an excitation and the cavity photon, quantified by vacuum Rabi frequency, becomes comparable to or larger than the corresponding electronic transition frequency in a cavity, the system can enter an ultrastrong coupling regime, which has been experimentally observed. In this regime, the standard rotating-wave approximation is no longer valid and the antiresonant term of the interaction Hamiltonian starts to play an important role, giving rise to exciting effects in cavity QED. The Aharonov-Bohm (AB) effect is a fundamental quantum phenomenon that bears the significance of the nature of electromagnetic fields and potentials. Besides its fundamental significance in quantum theory, its importance for applications in interferometric devices is omnipresent. Recently, since the 2D materials have triggered immense interest, some work has been done to integrate the AB effect with the electronic and transport properties of 2D materials. This thesis consists of two parts. In the first part, the light-matter coupling between cyclotron transition and photon is theoretically investigated in some 2-D materials such as the monolayer MoS2, graphene and monolayer black phosphorene (BP) systems. The results show that, in these 2-D materials, the ultrastrong light-matter coupling can be achieved at a high filling factor of Landau levels. Furthermore, we show that, in contrast to the case for conventional semiconductor resonators, the MoS2 system shows a vacuum instability. In monolayer MoS2 resonator, the diamagnetic term can still play an important role in determining magnetopolariton dispersion which is different from monolayer graphene system. The diamagnetic term arises from electron-hole asymmetry which indicates that electron-hole asymmetry can influence the quantum phase transition. Meanwhile, we show that, similar with some other 2D materials such as graphene and MoS2, the monolayer BP system shows a vacuum instability. However, in contrast with other 2D materials, the BP system displays a large energy gap between three branches of polaritons because of its strong anisotropic behavior in the eigenstates of the band structures. For the graphene system, we investigate the coupling of cyclotron transition and a multimode cavity described by a multimode Dicke model. This model exhibits a superradiant quantum phase transition, which we describe exactly in an effective Hamiltonian approach. The complete excitation spectrum in both the normal phase and superradiant phase regimes is given. At last, in contrast to the single mode case, multimode coupling of cavity photon and cyclotron transition can greatly reduce the critical vacuum Rabi frequency required for quantum phase transition, and dramatically enhance the superradiant emission by fast modulating the Hamiltonian. Our study provides new insights in cavity-controlled magneto-transport in these 2-D systems, which could lead to the development of polariton-based devices. The second part is a diversion from the main content of this thesis; readers who are not interested in foundational issues of physics can skip this part. For one charged quantum particle P moving in an electromagnetic vector potential Aˆµ = ( φˆ, - Aˆ ) created by some other charged particles, we can either use the framework of one particle quantum mechanics (OPQM) to calculate the evolutions of P, or we can treat this as an multi-particles problem in the framework of quantum field theory and calculate the evolution of P. These two methods need to be equivalent, i.e., they produce the same result for the evolution of P. One open question is how to describe the evolution of P within the framework of quantum field theory and show that these two methods yield the same result? In chapter 5, we are going to derive the OPQM from the quantum field theory, i.e., the quantum electrodynamics (QED) to be specific. We start with the discussions on the AB effect then raise a plausible interpretation within the QED framework. We provide a quantum treatment of the source of the electromagnetic potential and argue that the underlying mechanism in AB effect can be viewed as interactions between electrons described by QED theory where the interactions are mediated by virtual photons. On further analysis, we show that the framework of one particle quantum mechanics (OPQM) can be given, in general, as a mathematically approximated model which is reformulated from QED theory while the AB effect scheme provides a platform for our derivations. In addition, the classical Maxwell equations are derived from QED scattering process while both classical electromagnetic fields and potentials serve as mathematical tools that are constructed to approximate the interactions among elementary particles described by QED physics. This work opens up a new perspective on the nature of electromagnetic fields and potentials.
Understanding physical properties of quantum emitters strongly interacting with quantized electromagnetic modes is one of the primary goals in the emergent field of waveguide quantum electrodynamics (QED). When the light-matter coupling strength is comparable to or even exceeds energies of elementary excitations, conventional approaches based on perturbative treatment of light-matter interactions, two-level description of matter excitations, and photon-number truncation are no longer sufficient. Here we study in and out of equilibrium properties of waveguide QED in such nonperturbative regimes on the basis of a comprehensive and rigorous theoretical approach using an asymptotic decoupling unitary transformation. We uncover several surprising features ranging from symmetry-protected many-body bound states in the continuum to strong renormalization of the effective mass and potential; the latter may explain recent experiments demonstrating cavity-induced changes in chemical reactivity as well as enhancements of ferromagnetism or superconductivity. To illustrate our general results with concrete examples, we use our formalism to study a model of coupled cavity arrays, which is relevant to experiments in superconducting qubits interacting with microwave resonators or atoms coupled to photonic crystals. We examine the relation between our results and delocalization-localization transition in the spin-boson model; notably, we point out that a reentrant transition can occur in the regimes where the coupling strength becomes the dominant energy scale. We also discuss applications of our results to other problems in different fields, including quantum optics, condensed matter physics, and quantum chemistry.
The field of Polaritonic Chemistry studies molecules strongly coupled to the light field of optical cavities. The resulting modification of the potential energy landscape has been demonstrated to enable control over the chemical and physical properties of materials and molecular ensembles. This thesis extends the Tavis–Cummings model to describe molecules under strong light–matter coupling, incorporating static dipole moments and dipole self-energy contributions derived from the Pauli–Fierz Hamiltonian. These additional terms are shown to be essential for reproducing cavity-modified molecular dynamics and spectra. Simulations on the nuclear wavefunction propagation of MgH+ molecules demonstrate the impact of these terms, while an effective two-level system model accurately captures the behavior of large ensembles. Beyond single excitations, the thesis also explores the higher excitation manifolds of the Tavis-Cummings model, which reveals that allowing for more than a single excitation makes the reaction of the involved polaritons entropically more favorable. Open-system simulations highlight how the coherence of the system's initial state governs decay pathways and enables long-lived energy storage. Finally, a multilevel vibrational model coupled to a two-mode cavity is introduced, where a Raman scheme enables selective mixing of vibrational states. The simulation results show that continuous pumping can drive molecules into specific vibrational states while suppressing electronic excitation, both for single molecules and small ensembles. Together, these results provide new theoretical insights into the mechanisms by which optical cavities reshape molecular energy landscapes. The results suggest approaches for controlling photonic, electronic, and vibrational dynamics in strongly coupled systems, contributing to the theoretical foundation of polariton chemistry.
Dressing quantum states of matter with virtual photons can create exotic effects ranging from vacuum-field modified transport to polaritonic chemistry, and may drive strong squeezing or entanglement of light and matter modes. The established paradigm of cavity quantum electrodynamics focuses on resonant light-matter interaction to maximize the coupling strength ΩR/ωc, defined as the ratio of the vacuum Rabi frequency and the carrier frequency of light. Yet, the finite oscillator strength of a single electronic excitation sets a natural limit to ΩR/ωc. Here, we demonstrate a new regime of record-strong light-matter interaction which exploits the cooperative dipole moments of multiple, highly non-resonant magnetoplasmon modes specifically tailored by our metasurface. This multi-mode coupling creates an ultrabroadband spectrum of over 20 polaritons spanning 6 optical octaves, vacuum ground state populations exceeding 1 virtual excitation quantum for electronic and optical modes, and record coupling strengths equivalent to ΩR/ωc=3.19. The extreme interaction drives strongly subcycle exchange of vacuum energy between multiple bosonic modes akin to high-order nonlinearities otherwise reserved to strong-field physics, and entangles previously orthogonal electronic excitations solely via vacuum fluctuations of the common cavity mode. This offers avenues towards tailoring phase transitions by coupling otherwise non-interacting modes, merely by shaping the dielectric environment.
Cavity quantum electrodynamics (QED) is the study of the interaction between light conned in a microcavity and material modes (such as single atoms or electrons in quantum wells), where the quantum nature of light is crucial.This thesis theoretically examines four dierent systems where light becomes strongly coupled with dierent material modes leading to dierent eects stemming from the dierent dimensionality and natures of the systems.The rst system consists of a semiconductor slab embedded into a zero-dimensional microcavity, leading to vacuum band gap opening of the electron dispersion caused by the interactions with the cavity photon mode.The second system is a quantum ring coupled to polarized light, calculated non-perturbatively.Since the polarization breaks time reversal symmetry, the particles in the ring will exhibit an energy dierence of particles with the same magnitude of angular momentum but dierent directions.The viability of these resulting in Aharonov-Bohm oscillations in large rings is considered.The third system consists of an array of quantum wires embedded into a planar microcavity.The inhomogeneity of the two directions along and perpendicular to the wires, coupled with the homogeneous two-dimensional photon mode, leads to an emergence of a hyperbolic region and many peculiar eects.The fourth and last work considers an algorithm to modify systems, leading to a ladder of equidistant energies.To illustrate, a radially symmetric nanoparticle with a hydrogenic impurity is analysed.The material composition along the radius can be altered to achieve a cascade of transitions in the Terahertz range.When multiple such particles are embedded into a resonant microcavity, one can convert photons of a higher energy to multiple Terahertz photons.
Recent technological developments have made it increasingly easy to access the non-perturbative regimes of cavity quantum electrodynamics known as ultrastrong or deep strong coupling, where the light-matter coupling becomes comparable to the bare modal frequencies. In this work, we address the adequacy of the broadly used single-mode cavity approximation to describe such regimes. We demonstrate that, in the non-perturbative light-matter coupling regimes, the single-mode models become unphysical, allowing for superluminal signalling. Moreover, considering the specific example of the quantum Rabi model, we show that the multi-mode description of the electromagnetic field, necessary to account for light propagation at finite speed, yields physical observables that differ radically from their single-mode counterparts already for moderate values of the coupling. Our multi-mode analysis also reveals phenomena of fundamental interest on the dynamics of the intracavity electric field, where a free photonic wavefront and a bound state of virtual photons are shown to coexist.